Chemical Bond Breaking and the Role of Cavities in Solution Studied Using Femtosecond Spectroscopy and Mixed Quantum/Classical Molecular Dynamics Simulation

该奖项由化学系实验物理化学计划资助，加州大学洛杉矶分校的Benjamin J. Schwartz教授及其博士后和研究生同事将进行实验和理论相结合的研究计划，通过研究简单的原型模型系统，更好地了解溶液中的电子转移和光解反应。理论工作将集中在分子动力学模拟上，结合了Schwartz和他的同事开发的严格的混合量子/经典方法（包括组态相互作用），并将重点放在原子电子转移反应上，并初步研究简单双原子分子的光解，如碱金属二聚体或二聚体。模拟将补充碘离子和碱金属阴离子电荷转移到溶剂系统的电子转移反应的超快光谱测量。这些结果应该广泛适用于各种各样的溶液相系统，无论电子转移和相关的化学反应发生在哪里。除了支持研究的更广泛的科学影响外，参与该项目的年轻研究人员将同时获得前沿理论和实验方法的经验。

In this award, funded by the Experimental Physical Chemistry Program of the Chemistry Division, Prof. Benjamin J. Schwartz of the University of California, Los Angeles and his postdoctoral and graduate student colleagues will undertake a combined experimental and theoretical program of research to develop a better understanding of electron transfer and photodissociation reactions in solution through the study of simple, prototypical model systems. The theoretical work will center on molecular dynamics simulations incorporating a rigorous, mixed quantum/classical method (including configuration interaction) that Schwartz and his colleagues have developed, and will focus both on on atomic electron transfer reactions and preliminarily on the photodissociation of simple diatomic molecules such as alkali metal dimers or hydrides. The simulations will be complemented by ultrafast spectroscopy measurements of electron transfer reactions on iodide and alkali metal anion charge transfer to solvent systems. These results should be broadly applicable to a wide variety of solution-phase systems, wherever electron transfer and related chemical reactions take place.Besides the broader scientific impacts of the research being supported, the young researchers working on this project will gain simultaneous experience in both cutting edge theoretical and experimental methods.